Ternary zero-valent iron/phos photungstic acid/g-C3N4 composite (Fe-0@PTA/g-C3N4) was synthesized via photoreduction of iron (II) ions assisted by phosphotungstic acid (PTA) over g-C3N4 flakes. The as-prepared Fe-0@PTA/g-C3N4 was investigated for removal of As(III) and As(V) species from water. The result showed that Fe-0@PTA/g-C3N4 exhibited a better performance for As(V) removal than As(III) species from water, and the maximum adsorption capacity for As(V) was 70.3 mg/g, much higher than most of the reported adsorbents. As(V) removal by the Fe-0@PTA/g-C3N4 adsorbent is mainly via a chemical process, synergistically occurring of reduction of As(V) and oxidation of Fe-0. Moreover, the Fe-0@PTA/g-C3N4 adsorbent showed effective As(V) removal from the simulated industrial wastewater and underground water. This study demonstrates that Fe-0@PTA/g-C3N4 can be a potential adsorbent for As(V) removal due to its high performance, and simple one-pot synthesis process. (C) 2017 Elsevier B.V. All rights reserved.